Method for depositing silicon nitride films and silicon oxynitride films by chemical vapor deposition

ABSTRACT

A method for producing silicon nitride and silicon oxynitride films by CVD technology, where even at lower temperatures, acceptable film-deposition rates are achieved, without the by-product production of large amounts of ammonium chloride.

BACKGROUND OF THE INVENTION

This invention relates to methods for producing silicon nitride filmsand silicon oxynitride films by chemical vapor deposition (CVD).

Silicon nitride films exhibit excellent barrier properties and anexcellent oxidation resistance and for these reasons are used for, forexample, etch-stop layers, barrier layers, gate insulation layers, andONO stacks in the fabrication of microelectronic devices.

The main technologies in use at the present time for the formation ofsilicon nitride films are plasma-enhanced CVD (PECVD) and low-pressureCVD (LPCVD).

In PECVD, a silicon source (typically a silane) and a nitrogen source(typically ammonia but more recently nitrogen) are introduced between apair of parallel-plate electrodes and high-frequency energy is appliedbetween the two electrodes at low temperatures (about 300° C.) andintermediate pressures (0.1 to 5 Torr) in order to generate a plasmafrom the silicon source and nitrogen source. Active silicon species andactive nitrogen species in the generated plasma react with each other toproduce a silicon nitride film. The silicon nitride films produced byPECVD generally do not have a stoichiometric composition and are alsohydrogen rich. As a result, these silicon nitride films have a low filmdensity and a high etch rate and are of poor quality.

LPCVD, which does not employ a plasma, is used in order to deposithigh-quality silicon nitride films. LPCVD as it is currently practiceduses low pressures (0.1 to 2 Torr) and high temperatures (750-900° C.)and produces silicon nitride films of a quality superior to that of thesilicon nitride films produced by PECVD. Silicon nitride films havegenerally been produced by this LPCVD technology by the reaction ofdichlorosilane (DCS) and ammonia gas. However, the existing LPCVDtechnology requires fairly high temperatures in order to obtainacceptable deposition (film formation) rates (≧10 Å/minute) for siliconnitride films. For example, temperatures of 750 to 800° C. are typicallyused for the reaction of DCS and ammonia In addition, the reaction ofDCS and ammonia produces large amounts of ammonium chloride, which canaccumulate in and clog the exhaust plumbing system of the CVD reactionapparatus.

A number of silicon nitride precursors have been introduced for thepurpose of obtaining satisfactory silicon nitride film deposition ratesat low temperatures. Hexachlorodisilane (HCDS) is one example of suchprecursors. HCDS produces SiCl₂ at relatively low temperatures by thereaction Si₂Cl₆→SiCl₂+SiCl₄ and this SiCl₂ reacts well with ammonia Theuse of HCDS can provide silicon nitride film deposition at filmformation rates of approximately 10 Å/minute at 600° C.

Another example of these precursors is the is(tert-butylamino)silane(BTBAS) described in U.S. Pat. No. 5,874,368. Use of BTBAS can alsoprovide silicon nitride film deposition at lower temperatures than forthe use of DCS. As in the case of HCDS, BTBAS enables the deposition ofsilicon nitride films at a film formation rate of approximately 10Å/minute at 600° C.

While both HCDS and BTBAS can achieve film formation rates ofapproximately 10 Å/minute at 600° C., this performance level also meansthat commercially acceptable film formation rates will not be obtainedat lower temperatures ≦550° C., or in specific terms that a filmformation rate of at least 10 Å/minute will not be obtained at lowertemperatures ≦550° C. These two precursors are also associated with thedisadvantages described below.

HCDS, being a completely chlorinated disilane, has a high chlorinecontent, and the Si—Cl bond is also very strong. As a consequence, thechlorine content in the resulting silicon nitride film will increase asthe reaction temperature declines, and it has been found that thechlorine content reaches as high as about 2 atom % at a 600° C. reactiontemperature. In addition, HCDS also leads to the production of largeamounts of ammonium chloride just as in the case of DCS.

BTBAS has an activation energy of 56 kcal/mole, with the result that itssilicon nitride film formation rate declines drastically when thereaction temperature is reduced. It is estimated that its film formationrate drops to a quite small 3 Å/minute at a reaction temperature of 550°C.

The same problems appear when the aforementioned prior art precursorsare used to produce silicon oxynitride films, which have the samephysical properties and applications as silicon nitride films.

The issue addressed by this invention, therefore, is to provide a methodfor the production of silicon nitride and silicon oxynitride films byCVD technology, wherein said method provides acceptable film formationrates even at lower temperatures and is not accompanied by theproduction of large amounts of ammonium chloride.

SUMMARY

The first aspect of this invention provides a method for producingsilicon nitride films by chemical vapor deposition, said method beingcharacterized by

-   -   introducing a hydrocarbylaminodisilane compound with the general        formula        (R⁰)₃—Si—Si—(R⁰)₃  (I)        -   wherein            -   each R⁰ is independently selected from the hydrogen                atom, chlorine atom, and —NR¹(R² groups (wherein R¹ and                R² are each independently selected from the hydrogen                atom and C₁ to C₄ hydrocarbyl with the proviso that R¹                and R¹ may not both be the hydrogen atom) and at least                one R⁰ is the —NR¹(R²) group        -   and a nitrogen-containing gas selected from the group            consisting of ammonia, hydrazine, alkylhydrazine compounds,            and hydrogen azide into a reaction chamber loaded with at            least 1 substrate and    -   forming a silicon nitride film on the substrate by reacting the        hydrocarbylaminodisilane compound and nitrogen-containing gas at        a reaction temperature.

The second aspect of this invention provides a method for producingsilicon oxynitride films by chemical vapor deposition, characterized by

-   -   introducing a hydrocarbylaminodisilane compound with formula        (I), a nitrogen-containing gas selected from the group        consisting of ammonia, hydrazine, and hydrogen azide, and an        oxygen-containing gas selected from the group consisting of NO,        N₂O, NO₂, O₂, O₃, H₂O, and H₂O₂ into a reaction chamber loaded        with at least 1 substrate and    -   forming a silicon oxynitride film on the substrate by reacting        the hydrocarbylaminodisilane compound, nitrogen-containing gas,        and oxygen-containing gas at a reaction temperature.

BRIEF DESCRIPTION OF THE DRAWINGS

For a further understanding of the nature and objects for the presentinvention, reference should be made to the following detaileddescription, taken in conjunction with the accompanying drawings, inwhich like elements are given the same or analogous reference numbersand wherein:

FIG. 1 illustrates one embodiment of a CVD reaction apparatus that maybe used to create silicon oxynitride films as taught by the invention.

FIG. 2 illustrates another embodiment of a CVD reaction apparatus thatmay be used to create silicon nitride films as taught by the invention.

FIG. 3 contains the mass spectrum of the hexakis(monoethylamino)disilane as discussed in Example 1.

DESCRIPTION OF PREFERRED EMBODIMENTS

This invention will be explained in greater detail in the following.

This invention uses special compounds as precursors for silicon nitrideand silicon oxynitride (collectively referred to below as silicon(oxy)nitride) in the formation of silicon nitride films and siliconoxynitride films (collectively referred to below as silicon (oxy)nitridefilms) on substrates by thermal CVD technology.

The silicon (oxy)nitride precursors used in this invention arehydrocarbylaminodisilane compounds with formula (I).(R⁰)₃—Si—Si—(R⁰)₃  (I)

Each R⁰ in (I) is independently selected from the hydrogen atom,chlorine atom, and the —NR¹(R²) group and at least one group R⁰ must bethe —NR¹(R²) group. R¹ and R² in the —NR¹(R²) group are eachindependently selected from the hydrogen atom and C₁ to C₄ hydrocarbylwith the proviso that R¹ and R² may not both be the hydrogen atom. TheC₁ to C₄ hydrocarbyl includes vinyl and C₁ to C₄ alkyl such as methyl,ethyl, propyl, isopropyl, butyl, and tert-butyl.

Compounds in which each R⁰ is —NR¹(R²), R¹ is the hydrogen atom, and R²is C₁ to C₄ hydrocarbyl, that is, hexakis(monohydrocarbylamino)disilaneswith formula (II)((R)HN)₃—Si—Si—(NH(R))₃  (II)(each R independently represents C₁ to C₄ hydrocarbyl) are novelcompounds and are preferred compounds within the scope of thisinvention.

Hexakis(monohydrocarbylamino)disilanes with formula (II) can besynthesized by reacting hexachlorodisilane (Cl₃—Si—Si—Cl₃) in organicsolvent with at least 6-fold moles of the monohydrocarbylamine RNH₂(R=C₁ to C₄ hydrocarbyl). The monohydrocarbylamine for reaction withhexachlorodisilane includes, inter alia, methylamine, ethylamine,propylamine, isopropylamine, tert-butylamine, and vinylamine. Themonohydrocarbylamine used can take the form of a singlemonohydrocarbylamine or a mixture of monohydrocarbylamines. However, theuse of a single monohydrocarbylamine is preferred viewed from theperspective of ease of production, and the use of ethylamine is evenmore preferred.

As specified above, the hexachlorodisilane and monohydrocarbylamine arereacted with each other using at least 6 moles of the latter per 1 moleof the former. However, the use of a large excess of themonohydrocarbylamine over hexachlorodisilane is preferred for thepurpose of inhibiting the production of N-hydrocarbyldisilazane. Inspecific terms, the use of a hexachlorodisilane:monohydrocarbylaminemolar ratio of 1:12 to 1:36 is preferred. Use of at least 12 molesmonohydrocarbylamine per 1 mole hexachlorodisilane also enablestrapping, as the monohydrocarbylamine hydrochloride (solid), of thehydrogen chloride (6 moles) that is produced as a by-product in thereaction. This monohydrocarbylamine hydrochloride can be easily removedfrom the reaction mixture post-reaction by filtration.

Organic solvent is used as the reaction solvent for reaction of thehexachlorodisilane and monohydrocarbylamine. This organic solventencompasses tetrahydrofuran and straight-chain and cyclic hydrocarbons,for example, pentane, hexane, and octane. Pentane is the preferredsolvent.

The reaction between hexachlorodisilane and monohydrocarbylamine ispreferably run at a temperature from −30° C. to +50° C. In general, thisreaction will be run by first bringing the reaction solvent to atemperature in the preferred range of −30° C. to +50° C., introducingthe monohydrocarbylamine into the reaction solvent and dissolving ittherein, and then gradually adding the hexachlorodisilane, for example,by dropwise addition. The hexachlorodisilane can be dropped in eitherneat or dissolved in the same solvent as the reaction solvent. Thereaction is subsequently ran for 2 to 24 hours while stirring thereaction solvent and holding at the aforementioned temperature. Afterthis period of stirring, the reaction solvent is heated to roomtemperature (approximately 20° C. to 50° C.) and stirring is preferablycontinued for at least another 10 hours. The hydrocarbylammoniumchloride, a solid by-product, is then filtered off and the solvent andresidual amine are distilled off in vacuo. The resultinghexakis(monohydrocarbylamino)disilane can be subjected to additionalpurification by fractional distillation.

The hexakis(monohydrocarbylamino)disilanes (II) are liquids at ambienttemperatures (approximately 20° C. to 50° C.), do not contain chlorine,and are highly reactive and in particular support excellent silicon(oxy)nitride film formation rates at low temperatures (≦600° C.). Theirhigh reactivity is caused by the bonding of the monohydrocarbylaminogroup to the silicon and by the weak Si—Si direct bond.Hexakis(monoethylamino)disilane is a particularly preferredhexakis(monohydrocarbylamino)disilane (II).

In order to form silicon nitride using the inventivehydrocarbylaminodisilane compounds (I), the hydrocarbylaminodisilanecompound (I) and nitrogen-containing gas are admitted into a reactionchamber loaded with at least 1 substrate (typically a semiconductorsubstrate such as a silicon substrate) and silicon nitride is depositedon the semiconductor substrate by reacting the hydrocarbylaminodisilanecompound and nitrogen-containing gas at the reaction temperature. Thenitrogen-containing gas can be selected from the group consisting ofammonia, hydrazine, alkylhydrazine compounds, and hydrogen azide.

The molar ratio between the hydrocarbylaminodisilane compound andnitrogen-containing gas admitted into the reaction chamber duringsilicon nitride production is preferably 1:0 to 1:50. The total pressurewithin the reaction chamber is preferably maintained at from 0.1 to 10Torr. The reaction temperature is preferably from −300° C. to 650° C.

In order to form silicon oxynitride using the inventivehydrocarbylaminodisilane compounds (I), the hydrocarbylaminodisilanecompound (I), nitrogen-containing gas, and oxygen-containing gas areadmitted into a reaction chamber loaded with at least one substrate(typically a semiconductor substrate such as a silicon substrate) and asilicon oxynitride film is deposited on the substrate by reacting thehydrocarbylaminodisilane compound, nitrogen-containing gas, andoxygen-containing gas at the reaction temperature. As with siliconnitride film deposition, the nitrogen-containing gas can be selectedfrom the group consisting of ammonia, hydrazine, and hydrogen azide. Theoxygen-containing gas can be selected from the group consisting of NO,N₂O, NO₂, O₂, O₃, H₂O, and H₂O₂.

When the oxygen-containing gas also contains nitrogen (NO, N₂O, and/orNO₂), the nitrogen-containing gas need not be used and the ratio betweenthe hydrocarbylaminodisilane compound and the nitrogen-containing gasadmitted into the reaction chamber during silicon oxynitride productionis preferably 1:0 to 1:50. When the oxygen-containing gas does notcontain nitrogen (O₂, O₃, H₂O, and/or H₂O₂), the molar ratio between thehydrocarbylaminodisilane compound and the nitrogen-containing gas ispreferably 10:1 to 1:50. In either case the molar ratio between thehydrocarbylaminodisilane compound and oxygen-containing gas ispreferably 50:1 to 1:10. The overall pressure within the reactionchamber is preferably maintained in the range from 0.1to 10 Torr, andthe reaction temperature is preferably −300° C. to 750° C.

The hydrocarbylaminodisilane compound (I) can be vaporized using abubbler or a vaporizer during silicon (oxy)nitride production accordingto this invention. The bubbler can comprise a sealed container filledwith liquid hydrocarbylaminodisilane compound (I), an injection conduitthat injects carrier gas into the hydrocarbylaminodisilane compound inthe sealed container, and a feed conduit that removeshydrocarbylaminodisilane compound—vaporized and entrained into thecarrier gas injected from the injection conduit into thehydrocarbylaminodisilane compound—from the sealed container and feedsthis vaporized hydrocarbylaminodisilane compound into the reactionchamber. At its downstream end this feed conduit communicates with theCVD reaction chamber. The temperature and pressure within the sealedcontainer must be maintained at constant or specified values.

A Direct Liquid Injection System (DLI-25) from the MKS Company or aVU-410A vaporizer from the Lintec Company, for example, can be used asthe vaporizer. The hydrocarbylaminodisilane compound is vaporized usingthe vaporizer and fed to the reaction chamber.

FIG. 1 contains a block diagram that illustrates one example of a CVDreaction apparatus well suited for execution of the inventive method forproducing silicon (oxy)nitride films.

The CVD reaction apparatus 10 illustrated in FIG. 1 is provided with aCVD reaction chamber 11, a supply source 12 for thehydrocarbylaminodisilane compound (HCAD) according to this invention, anitrogen-containing gas supply source 13, and a supply source 14 ofdilution gas, such as an inert gas, that is introduced as necessary. TheCVD reaction apparatus 10 is also provided with an oxygen-containing gassupply source 15 when silicon oxynitride is to be produced The reactionchamber 11 is surrounded by a heating means 111 for the purpose ofheating to the specified CVD reaction temperature (batch processing). Asusceptor is heated in the case of single wafer processing.

In the case of the CVD reaction apparatus 10 illustrated in FIG. 1, theHCAD is introduced into the reaction chamber 11 in the gas phase due to.the action of a bubbler. The HCAD supply source 12 is provided with asealed container 121 that is loaded with liquid HCAD. An injectionconduit 122 is inserted into the sealed container 121 in order to injectcarrier gas into the HCAD loaded in the sealed container 121; thecarrier gas is injected from the supply source 16 for the carrier gas,e.g., nitrogen, across the valve V1 and mass flow controller MFC1. Afterits injection into the HCAD, the HCAD-entraining carrier gas passesthrough the pressure-control valve PV and into the line L1 and isintroduced into the reaction chamber 11. A pressure sensor PG1 isconnected to the line L1 Although not shown in the figure, at least 1substrate (typically a semiconductor substrate such as a siliconsubstrate) is loaded in the reaction chamber 11. From 1 to 250substrates (chuck- or wafer boat-loaded) can be present

Nitrogen-containing gas, e.g., ammonia, is introduced from thenitrogen-containing gas supply source 13 across the valve V2 and themass flow controller MFC2 and into the reaction chamber 11 through theline L2.

Dilution gas, which is introduced as necessary, can be introduced fromthe dilution gas supply source 14 across the valve V3 and the mass flowcontroller MFC3 and into the reaction chamber 11 through the line L3 andthe line L2.

Oxygen-containing gas, which is introduced during production of siliconoxynitride films, can be introduced from the oxygen-containing gassupply source 15 across the valve V4 and the mass flow controller MFC4and into the reaction chamber 11 through the line L4 and the line L2.

The outlet from the reaction chamber 11 is connected by the line L5 to awaste gas treatment apparatus 17. This waste gas treatment apparatus 17functions to remove, for example, by-products and unreacted material,and to -exhaust the gas after abatement from the system. A pressuresensor PG2, a butterfly valve BV, and a pump PM are connected in theline L5. The various gases are introduced into the reaction chamber 11,the pressure within the reaction chamber 11 is monitored by the pressuresensor PG2, and the pressure is brought to its prescribed value by theopening and closing of the butterfly valve BV by the operation of thepump PM.

During operation, the container 121 is heated to, for example, 50° C. to80° C., and the HCAD feed system, which comprises the line L1, ispreferably heated to a temperature higher than the bubbler in order toprevent dew formation by the HCAD.

FIG. 2 contains a CVD reaction apparatus that has the same structure asthe CVD reaction apparatus 10 illustrated in FIG. 1, with the exceptionthat the CVD reaction apparatus in FIG. 2 contains a different HCAD feedsystem. Those elements that are the same in both figures have beenassigned the same reference symbol and will not be considered again indetail.

The CVD reaction apparatus 20 illustrated in FIG. 2 is provided with avaporizer 21. Carrier gas from the carrier gas source 16 passes acrossthe valve V1 and through the line L21 and is introduced into thegas-phase region for the HCAD filled in liquid form in the sealedcontainer 22. The pressure exerted by the carrier gas functions to movethe liquid HCAD across the valve V22 and the mass flow controller MFC21,through the line L22, and into the vaporizer 21. Carrier gas from thecarrier gas source 16 also passes through the line L22, which branchesfrom the line L21, and is introduced into the vaporizer 21. The carriergas and liquid HCAD introduced into the vaporizer 21 are heated in thevaporizer 21 to, for example, 60° C. to 200° C., and the HCAD isvaporized and is transported with the carrier gas through the line L23and is introduced into the reaction chamber 11. The line L23 ispreferably heated to 50° C. to −250° C. in order to preventreliquefaction or dew formation by the HEAD.

EXAMPLES

This invention is described in greater detail in the following throughworking examples, but the invention is not limited to these examples.

Synthesis Example 1 Synthesis of Hexakis(monoethylamino)disilane (HEAD)

Pentane was used as the reaction solvent and was cooled to 0° C. for thereaction. An ethylamine solution was prepared by adding ethylamine (70g, 1.55 mol) cooled to 0° C. to the cold pentane. Hexachlorodisilane(26.9 g, 0.1 mol) was gradually added to this ethylamine solution. Theresulting reaction solution was thereafter stirred for 2 hours at 0° C.and then for an additional 15 hours at room temperature (20° C.). Theethylamonium-chloride by-product was filtered off and the pentane andethylamine were distilled out in vacuo. 22.4 g HEAD was obtained(yield=70%).

Results of Analysis

¹H-NMR (C₆D₆, 500 MHz): δ=0.61 ppm (broad, —NH), δ=1.1 ppm (triplet,—CH₃), δ(pentet, —CH₂)

¹³C-NMR (C₆D₆, 125 MHz): 20.7 ppm and 36.1 ppm (—CH₂CH₃)

A signal assignable to the SiH bond was not observed in these NMRanalyses.

FIG. 3 reports the analytical results (spectrum) from QMS (m/e<250)(Et=ethyl in FIG. 3). While the Si—Si bond was present in a number offragments, for the sake of simplicity assignments are given only formain peaks.

The chlorine content of the synthesized HEAD product, as measured by ionchromatography, was no greater than trace levels. The melting point ofthe HEAD product was estimated-about 10 C.

Example 1 Deposition of Silicon Nitride Film

A silicon nitride film was deposited in this example on a siliconsemiconductor substrate using a CVD reaction apparatus that had the samestructure as the CVD reaction apparatus in FIG. 2. The HEAD synthesizedin Synthesis Example 1 was used as the HCAD; ammonia was used as thenitrogen-containing gas; and nitrogen was used as the carrier gas. Theconditions listed below were used to produce the silicon nitride film.The line L23 was heated to 110° C. during -deposition.

-   HEAD gas flow rate: 5 sccm-   ammonia gas flow rate: 50 sccm-   carrier gas (nitrogen) flow rate: 60 sccm-   pressure within the reaction chamber: 0.5 Torr-   reaction chamber temperature: 550° C.-   vaporizer temperature: 110° C.

A silicon nitride film with a thickness of 900 Å was obtained in about45 minutes as a result (silicon nitride film deposition rate=20Å/minute). This silicon nitride film had a composition of Si_(1.5)N₁according to analysis by Auger electron spectroscopy.

Using conditions that were otherwise the same as those listed above,silicon nitride films were fabricated using reaction chambertemperatures of 500° C. and 525° C. Silicon nitride films were obtainedat deposition rates of 10 Å/minute and 15 Å/minute, respectively.

Example 2 Deposition of Silicon Oxynitride Film

A silicon oxynitride film was deposited in this example on a siliconsemiconductor substrate using a CVD reaction apparatus that had the samestructure as the CVD reaction apparatus in FIG. 2. The HEAD synthesizedin Synthesis Example 1 was used as the HCAD; ammonia was used as thenitrogen-containing gas; oxygen was used as the oxygen-containing gas;and nitrogen was used as the carrier gas. The conditions listed belowwere used to produce the silicon oxynitride film. The line L23 washeated to 110° C. during production.

-   HEAD gas flow rate: 2 sccm-   ammonia gas flow rate: 50 sccm-   oxygen flow rate: 1 sccm-   carrier gas (nitrogen) flow rate: 60 sccm-   pressure within the reaction chamber: 0.5 Torr-   reaction chamber temperature: 550° C.-   vaporizer temperature: 110° C.

A silicon oxynitride film with a thickness of approximately 2,000 Å wasobtained in about 100 minutes as a result (silicon oxynitride filmdeposition rate=20 Å/minute). This silicon oxynitride film had acomposition of SiN_(0.42)O_(0.35) according to analysis by Augerelectron spectroscopy.

As has been described in the preceding, this invention enables thedeposition of silicon nitride and silicon oxynitride films by CVDtechnology at satisfactory film formation rates even at low temperaturesand does so without being accompanied by the deposition of large amountsof ammonium chloride.

Example 3 Production of Silicon Nitride Film

A silicon nitride film was deposited in this example on a siliconsemiconductor substrate using a CVD reaction apparatus that had the samestructure as the CVD reaction apparatus in FIG. 2. The HEAD synthesizedin Synthesis Example 1 was used as the HCAD; no nitrogen-containing gaswas introduced, and nitrogen was used as the carrier gas. The conditionslisted below were used to produce the silicon nitride film. The line L23was heated to 110° C. during production.

-   HEAD gas flow rate: 1.5 sccm-   carrier gas (nitrogen) flow rate: 15 sccm-   pressure within the reaction chamber: 1 Torr-   reaction chamber temperature: 450° C.-   vaporizer temperature: 110° C.    A silicon nitride film with a thickness of about 1250 Å was obtained    in about 150 minutes as a result (silicon nitride film deposition    rate=about 8 Å/minute). According to Auger electron spectroscopy the    Si to N ratio is about 1.5

REFERENCE SYMBOLS

-   -   10, 20 . . . CVD reaction apparatus    -   11 . . . CVD reaction chamber    -   12 . . . hydrocarbylaminodisilane (HCAD) supply source    -   13 . . . nitrogen-containing gas supply source    -   14 . . . dilution gas supply source    -   15 . . . oxygen-containing gas supply source    -   16 . . . carrier gas supply source    -   17 . . . waste gas treatment apparatus    -   21 . . . vaporizer    -   22 . . . sealed container    -   111 . . . heating means    -   121 . . . sealed container    -   122 . . . carrier gas injection conduit    -   L1-L5, L21-L23 . . . line    -   V1-V4, V21-V22 . . . valve    -   PG1-PG2 . . . pressure sensor    -   MFC1-MFC4, MFC21-MFC22 . . . mass flow controller    -   BV . . . butterfly valve    -   PM . . . pump

It will be understood that many additional changes in the details,materials, steps and arrangement of parts, which have been hereindescribed in order to explain the nature of the invention, may be madeby those skilled in the art within the principle and scope of theinvention as expressed in the appended claims. Thus, the presentinvention is not intended to be limited to the specific embodiments inthe examples given above.

1. A method for producing silicone nitride films comprising: a)introducing into a reaction chamber, said chamber containing at leastone substrate; i) a hydrocarbylaminodisilane compound with generalformula (I)(R⁰)₃—Si—Si—(R⁰)₃ (I)  wherein each R⁰ is independently selected fromthe group consisting of: a hydrogen atom, a chlorine atom, and a—NR¹(R²) group,  wherein at least one R⁰ is said —NR¹(R²) group; whereinsaid —NR^(1(R) ²) group further comprises R¹ and R² being eachindependently selected from the group consisting of: a hydrogen atom;and a C₁ to C₄ hydrocarbyl, and wherein only one said R¹ or R² is ahydrogen atom, and ii) a nitrogen-containing gas; and b) reacting saidcompound and said gas.
 2. The method of claim 1, wherein said gascomprises at least one member selected from the group consisting of: a)ammonia; b) hydrazine; c) alklhydrazine compounds; and d) hydrogenazide.
 3. The method of claim 1, further comprising saidhydrocarbylaminodisilane compound of general formula (I)(R⁰)₃—Si—Si—(R⁰)₃  (I) wherein each R⁰ is the —NR¹(R²) group, R¹ is ahydrogen atom, and R² is a C₁ to C₄ hydrocarbyl.
 4. The method of claim1, wherein said compound contains hexakis(ethylamino)disilane.
 5. Themethod of claim 1, wherein the molar ratio between said compound andsaid gas is in the range of about 1:0 to about 1:50.
 6. The method ofclaim 1, wherein the pressure within said reaction chamber is in therange of about 0.1 Torr to about 10 Torr.
 7. The method of claim 1,wherein the reaction temperature is in the range of about −300C to about650° C.
 8. The method claim of 1, wherein the molar ration between saidcompound and said gas is in the range of about 1:0 to about 1:50; thepressure within said reaction chamber is in the range of about 0.1 Torrto about 10 Torr; and the reaction temperature is in the range of about−300° C. to about 650° C.
 9. The method of claim 1, further comprising:a) injecting a carrier gas into the liquid form of saidhydrocarbylaminodisilane compound; b) entraining said compound as a gasin said carrier gas; c) moving said entrained compound through the feedsystem; and d) feeding said entrained compound into said reactionchamber.
 10. The method of claim 9, wherein the temperature of said feedsystem is in the range of about −250° C. to about 25°C.
 11. The methodof claim 1, further comprising: a) vaporizing said compound using avaporizer; b) moving said vaporized compound through the feed system;and c) feeding said vaporized compound into said reaction chamber. 12.The method of claim 11, wherein the temperature of said vaporizer is inthe range of about 60° C. to about 200° C.
 13. The method of claim 10,wherein the temperature of said feed system is in the range of about−250° C. to about 25° C.
 14. The method of claim 1, further comprising:a) loading said reaction chamber with a quantity of semiconductorsubstrates; and b) mounting said substrates in one chuck or wafer boat.15. The method of claim 14, wherein said quantity is in the range ofabout 1 to about
 250. 16. A method for producing silicone oxynitridefilms comprising: a) introducing into a reaction chamber, said chambercontaining at least one substrate; i) a hydrocarbylaminodisilanecompound with general formula (I)(R⁰)₃—Si—Si—(R⁰)₃  (I)  wherein each R⁰ is independently selected fromthe group consisting of: a hydrogen atom, a chlorine atom, and a—NR¹(R²) group,  wherein at least one R⁰ is the —NR¹(R²); wherein said—NR¹(R²) group further comprises R¹ and R²; wherein said R¹ and R²areeach independently selected from the group consisting of: a hydrogenatom, and a C₁ to C₄ hydrocarbyl; and wherein only R¹ or R² is saidhydrogen atom; and ii) a nitrogen-containing gas, iii) anoxygen-containing gas, and b) reacting said compound, saidnitrogen-containing gas, and said oxygen-containing gas.
 17. The methodof claim 16, wherein said nitrogen-containing gas comprises at least onemember selected from the group consisting of: a) ammonia; b) hydrazine;c) alklhydrazine compounds; and d) hydrogen azide.
 18. The method ofclaim 16, wherein said oxygen-containing gas comprises at least onemember selected from the group consisting of: a) nitric oxide; b)nitrous oxide; c) nitrogen peroxide; d) oxygen; e) ozone; f) watervapor; and g) hydrogen peroxide.
 19. The method of claim 16, furthercomprising said compound of general formula (I)(R⁰)₃—Si—Si—(R⁰)₃  (I) wherein each R⁰ is the —NR^(1(R) ²) group, R¹ isa hydrogen atom, and R^(2 is a C) ₁ to C₄ hydrocarbyl.
 20. The method ofclaim 16, wherein said compound comprises hexakis(ethylamino)disilane.21. The method of claim 16, wherein the molar ratio between saidcompound and said nitrogen-containing gas is in the range of about 1:0to about 1:50.
 22. The method of claim 16, wherein the molar ratiobetween said compound and said oxygen-containing gas is in the range ofabout 50:1 to about 1:10.
 23. The method of claim 16, wherein thepressure within said reaction chamber is in the range of about 0.1 Torrto about 10 Torr.
 24. The method of claim 16, wherein the reactiontemperature is in the range of about −300C to about 750° C.
 25. Themethod of claim 16, wherein the molar ratio between said compound andsaid nitrogen-containing gas is in the range of about 1:0 to about 1:50,the molar ratio between said compound and said oxygen-containing gas isin the range of about 50:1 to about 1:10, the pressure within saidreaction chamber is in the range of about 0.1 Torr to about 10 Torr, andthe reaction temperature is in the range of about −300° C. to about 750°C.
 26. The method of claim 16, further comprising: a) injecting acarrier gas into the liquid form of said compound; b) entraining saidcompound as a gas in said carrier gas; c) moving said entrained compoundthrough the feed system; and d) feeding said entrained compound intosaid reaction chamber.
 27. The method of claim 26, wherein thetemperature of said feed system is in the range of about 25° C. to about−250° C.
 28. The method of claim 16, further comprising: a) vaporizingsaid compound using a vaporizer; b) moving said vaporized compoundthrough said feed system; and c) feeding said vaporized compound intosaid reaction chamber.
 29. The method of claim 28, wherein thetemperature of said feed system is in the range of about 25° C. to about−250° C.
 30. The method of claim 16, wherein the temperature of saidvaporizer is in the range of about 60° C. to about 200° C.
 31. Themethod of claim 16, further comprising: a) loading said reaction chamberwith a quantity of semiconductor substrates; and b) mounting saidsubstrates in one chuck or wafer boat.
 32. The method of claim 31,wherein said quantity is in the range of about 1 to about 250.